Skip to main content
SpringerLink
Log in

Effects of additives on palladium nanocrystals supported on multiwalled carbon nanotubes and their electrocatalytic properties toward formic acid oxidation

  • Original Paper
  • Published:
Ionics Aims and scope Submit manuscript

Abstract

Carbon nanotubes are believed to be powerful materials for constructing novel hybrid composites with desirable functionalities and applications in many fields. Therefore, a better understanding of the functionalization of multiwalled carbon nanotubes (MWCNTs) holds the key to a better performance of the hybrid properties. In this paper, with a series of aromatic bifunctional molecule additives, modified MWCNTs were used as composite supports for synthesizing nanostructured palladium catalysts for formic acid oxidation. The additives contain anthranilic acid, o-phenylenediamine, salicylic acid, catechol, and phthalic acid. The influence of the different bifunctional groups (such as –NH2, –OH, –COOH, and their mixed groups) on the morphologies, particle sizes, and electrical properties of Pd nanocrystals was intensively studied. Transmission electron microscopy measurement demonstrates that the palladium nanoparticles were well dispersed on the surface of MWCNTs with a relatively narrow particle size distribution in the presence of the additives. Cyclic voltammetry and chronoamperometry tests demonstrate that the functional groups of the additives play an important role in electrocatalytic activity and stability for formic acid oxidation, and the influence law of various functional groups on electrocatalytic activity and stability is also investigated in this paper. We hope it can provide certain theoretical guidance meaning and practical reference value in future studies.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  1. Antolini E, Salgado JRC, Gonzalez ER (2006) The methanol oxidation reaction on platinum alloys with the first row transition metals, the case of Pt–Co and –Ni alloy electrocatalysts for DMFCs: a short review. Appl Catal B: Environ 63:137–149

    Article  CAS  Google Scholar 

  2. Thomas JE, Bonesi AR, Moreno MS, Visintin A, Castro Luna AM, Triaca WE (2010) Carbon nanotubes as catalyst supports for ethanol oxidation. Int J Hydrog Energy 35:11681–11686

    Article  CAS  Google Scholar 

  3. Lim B, Jiang MJ, Camargo PHC, Cho EC, Tao J, Lu XM, Zhu YM, Xia YN (2009) Pd-Pt Bimetallic nanodendrites with high activity for oxygen reduction. Science 324:1302–1305

    Article  CAS  Google Scholar 

  4. Zhu YM, Ha SY, Masel RI (2004) High power density direct formic acid fuel cells. J Power Sources 130:8–14

    Article  CAS  Google Scholar 

  5. Kang SJ, Lee J, Lee JK, Chung SY, Tak Y (2006) Influence of Bi modification of Pt anode catalyst in direct formic acid fuel cells. J Phys Chem B 110:7270–7274

    Article  CAS  Google Scholar 

  6. Zhao J, Wang P, Chen WX, Liu R, Li X, Nie QL (2006) Microwave synthesis and characterization of acetate-stabilized Pt nanoparticles supported on carbon for methanol electro-oxidation. J Power Sources 160:563–569

    Article  CAS  Google Scholar 

  7. Wang RF, Li H, Feng HQ, Wang H, Lei ZQ (2010) Preparation of carbon-supported core@shell PdCu@PtRu nanoparticles for methanol oxidation. J Power Sources 195:1099–1102

    Article  CAS  Google Scholar 

  8. Casado-Rivera E, Volpe DJ, Alden L, Lind C, Downie C, Vazquez-Alvarez T, Angelo ACD, DiSalvo FJ, Abruna HD (2004) Electrocatalytic activity of ordered intermetallic phases for fuel cell applications. J Am Chem Soc 126:4043–4049

    Article  CAS  Google Scholar 

  9. Kang YJ, Qi L, Li M, Diaz RE, Su D, Adzic RR, Stach E, Li J, Murray CB (2012) Highly active Pt3Pb and core-shell Pt3Pb-Pt electrocatalysts for formic acid oxidation. ACS Nano 6:2818–2825

    Article  CAS  Google Scholar 

  10. Mazumder V, Sun SH (2009) Oleylamine-mediated synthesis of Pd nanoparticles for catalytic formic acid oxidation. J Am Chem Soc 131:4588–4589

    Article  CAS  Google Scholar 

  11. Bai ZY, Yang L, Li L, Lv L, Wang K, Zhan J (2009) A facile preparation of hollow palladium nanosphere catalysts for direct formic acid fuel cell. J Phys Chem C 113:10568–10573

    Article  CAS  Google Scholar 

  12. Liu ZL, Hong L, Tham MP, Lim TH, Jiang H (2006) Nanostructured Pt/C and Pd/C catalysts for direct formic acid fuel cells. J Power Sources 161:831–835

    Article  CAS  Google Scholar 

  13. Wang X, Tang YW, Gao Y, Lu TH (2008) Carbon-supported Pd–Ir catalyst as anodic catalyst in direct formic acid fuel cell. J Power Sources 175:784–788

    Article  CAS  Google Scholar 

  14. Uchida M, Aoyama Y, Tanabe M, Yanagihara N, Eda N, Ohta A (1995) Influences of both carbon supports and heat-treatment of supported catalyst on electrochemical oxidation of methanol. J Electrochem Soc 142:2572–2576

    Article  CAS  Google Scholar 

  15. Rajesh B, Karthik V, Karthikeyan S, Thampi KR, Bonard JM, Viswanathan B (2002) Pt–WO3 supported on carbon nanotubes as possible anodes for direct methanol fuel cells. Fuel 81:2177–2190

    Article  CAS  Google Scholar 

  16. Chen P, Zhang HB, Lin GD, Hong Q, Tsai KR (1997) Growth of carbon nanotubes by catalytic decomposition of CH4 or CO on a Ni-MgO catalyst. Carbon 35:1495–1501

    Article  CAS  Google Scholar 

  17. Zhou JM, Lin GD, Zhang HB (2009) Efficient growth of MWCNTs from decomposition of liquefied petroleum gas on a NixMg1-xO catalyst. Catal Commun 10:1944–1947

    Article  CAS  Google Scholar 

  18. Wu B, Hu D, Kuang K (2009) Functionalization of carbon nanotubes by an ionic-liquid polymer: dispersion of Pt and PtRu nanoparticles on carbon nanotubes and their electrocatalytic oxidation of methanol. Angew Chem Int Ed 48:4751–4754

    Article  CAS  Google Scholar 

  19. Britto PJ, Santhanam KSV, Ajayan PM (1996) Carbon nanotube electrode for oxidation of dopamine. Bioelectrochem Bioenerg 41:121–125

    Article  CAS  Google Scholar 

  20. Simmons TJ, Bult J, Hashim DP, Linhardt RJ, Ajayan PM (2009) Noncovalent functionalization as an alternative to oxidative acid treatment of single wall carbon nanotubes with applications for polymer composites. ACS Nano 3:865–870

    Article  CAS  Google Scholar 

  21. Wang SY, Wang X, Jiang SP (2008) PtRu nanoparticles supported on 1-aminopyrene-functionalized multiwalled carbon nanotubes and their electrocatalytic activity for methanol oxidation. Langmuir 24:10505–10512

    Article  CAS  Google Scholar 

  22. Bai ZY, Guo YM, Yang L, Li L, Hu CG (2011) Highly dispersed Pd nanoparticles supported on 1,10-phenanthroline-functionalized multi-walled carbon nanotubes for electrooxidation of formic acid. J Power Sources 196:6232–6237

    Article  CAS  Google Scholar 

  23. Suo Y, Hsing IM (2009) Size-controlled synthesis and impedance-based mechanistic understanding of Pd/C nanoparticles for formic acid oxidation. Electrochim Acta 55:210–217

    Article  CAS  Google Scholar 

  24. Zhou WJ, Lee JY (2008) Particle size effects in Pd-catalyzed electrooxidation of formic acid. J Phys Chem C 112:3789–3793

    Article  CAS  Google Scholar 

  25. Zhang S, Shao Y, Yin G, Lin Y (2010) Facile synthesis of PtAu alloy nanoparticles with high activity for formic acid oxidation. J Power Sources 195:1103–1106

    Article  CAS  Google Scholar 

  26. Liang HP, Lawrence NS, Jones TGJ, Banks CE, Ducati C (2007) Nanoscale tunable proton/hydrogen sensing: evidence for surface-adsorbed hydrogen atom on architectured palladium nanoparticles. J Am Chem Soc 129:6068–6069

    Article  CAS  Google Scholar 

  27. Zhou ZY, Kang XW, Song Y, Chen SW (2011) Butylphenyl-functionalized palladium nanoparticles as effective catalysts for the electrooxidation of formic acid. Chem Commun 47:6075–6077

    Article  CAS  Google Scholar 

  28. Wang XM, Xia YY (2009) Synthesis, characterization and catalytic activity of an ultrafine Pd/C catalyst for formic acid electrooxidation. Electrochim Acta 54:7525–7530

    Article  CAS  Google Scholar 

  29. Weaver MJ, Chang SC, Leung LW, Jiang X, Rubel M, Szklarczyk M, Zurawski D, Wieckowski A (1992) Evaluation of absolute saturation coverages of carbon monoxide on ordered low-index platinum and rhodium electrodes. J Electroanal Chem 327:247–260

    Article  CAS  Google Scholar 

  30. Zhao YC, Yang XL, Tian JN, Wang FG, Zhan L (2010) A facile and novel approach toward synthetic polypyrrole oligomers functionalization of multi-walled carbon nanotubes as PtRu catalyst support for methanol electro-oxidation. J Power Sources 195:4634–4640

    Article  CAS  Google Scholar 

  31. Chen YX, Heinen M, Jusys Z, Behm RJ (2007) Kinetic isotope effects in complex reaction networks: formic acid electro-oxidation. Chemphyschem 8:380–385

    Article  CAS  Google Scholar 

  32. Chen YX, Heinen M, Jusys Z, Behm RJ (2006) Kinetics and mechanism of the electrooxidation of formic acid—spectroelectrochemical studies in a flow cell. Angew Chem Int Ed 45:981–985

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This work was financially supported by the National Natural Science Foundation of China (grant nos. 21171051 and 61176004), Science and Technology Program of Henan Province (grant no. 112102210005), Basic and Frontier Research Program of Henan Province (grant no. 132300410016), and Science and Technology Foundation of He’nan Educational Committee (grant no. 12A150013).

Author information

Authors and Affiliations

  1. School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, Xinxiang, 453007, People’s Republic of China

    Huiying Yan, Zhengyu Bai, Shujun Chao, Qian Cui, Lu Niu, Lin Yang & Kai Jiang

  2. College of Environmental Science and Engineering, Donghua University, Shanghai, 201620, People’s Republic of China

    Jinli Qiao

Authors
  1. Huiying Yan
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Zhengyu Bai
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Shujun Chao
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Qian Cui
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Lu Niu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Lin Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Jinli Qiao
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Kai Jiang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Lin Yang or Jinli Qiao.

Additional information

Huiying Yan and Zhengyu Bai contributed equally to this work and should be considered co-first authors.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Yan, H., Bai, Z., Chao, S. et al. Effects of additives on palladium nanocrystals supported on multiwalled carbon nanotubes and their electrocatalytic properties toward formic acid oxidation. Ionics 20, 259–268 (2014). https://doi.org/10.1007/s11581-013-0962-6

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11581-013-0962-6

Keywords

Search

Navigation